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首页> 外文期刊>Journal of Electroanalytical Chemistry: An International Journal Devoted to All Aspects of Electrode Kinetics, Interfacial Structure, Properties of Electrolytes, Colloid and Biological Electrochemistry >Electrogenerated chemiluminescence of lucigenin enhanced by the modifications of electrodes with self-assembled monolayers and of solutions with surfactants
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Electrogenerated chemiluminescence of lucigenin enhanced by the modifications of electrodes with self-assembled monolayers and of solutions with surfactants

机译：通过修饰具有自组装单层的电极和具有表面活性剂的溶液，增强了光泽素的电化学发光

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摘要

Electrogenerated chemiluminescence (ECL) of lucigenin (Luc~(2+)·2NO_3~-, N,N'-dimethyl-9,9'-biacridinium dinitrate) in dioxygen-saturated alkaline aqueous solutions of pH 10 has been examined utilizing modifications of electrodes (i.e. self-assembled monolayer (SAM)-modified gold electrodes) and of solutions (i.e. micellar solutions containing a nonionic surfactant, Triton X-100) for the first time. In both cases of the modifications, enhanced ECL was observed, and the ECL was considered to be derived from the decomposition of a dioxetane-type intermediate formed by the radical-radical coupling reaction between an electrogenerated superoxide ion (O_2~(·-) and a one-electron reduced form of Luc~(2+) (i.e. a radical cation, Luc~(·+)). The surface modification of gold electrodes was achieved with dimercaptosuccinic acid (DMSA) and DL-thioctic acid (DL-TA) having carboxyl end groups. The amount of ECL at DL-TA-SAM-modified electrodes was about five times as that at the bare electrode. The enhancement of ECL at the SAM-modified electrodes would be due to the concentration effect of positively charged Luc~(2+) ions, the prevention of adsorption of the electrogenerated chemiluminescent product (i.e. N-methylacridone (NMA) and the two-electron reduced form of Luc~(2+) (Luc~0) on the electrode surfaces, and the effective generation of O_2~(·-). On the other hand, the amount of ECL in the micellar solution increased by about six times in comparison with that in the solution containing no surfactant. The enhanced ECL in micellar solutions would result mainly from the inhibition of adsorption of NMA and Luc~0 insoluble in water on electrode surfaces.
机译：荧光素（Luc〜（2+）·2NO_3〜-，N，N'-二甲基-9,9'-二氮cri啶鎓硝酸盐）在pH为10的双氧饱和碱性水溶液中的电化学发光（ECL）已通过电极（即自组装单层（SAM）修饰的金电极）和溶液（即包含非离子表面活性剂Triton X-100的胶束溶液）首次使用。在两种修改的情况下，均观察到增强的ECL，并且认为ECL源自电生超氧离子（O_2〜（·-）与电子之间的自由基自由基偶联反应形成的二氧杂环丁烷型中间体的分解。一种单电子还原形式的Luc〜（2 +）（即自由基阳离子，Luc〜（·+）），金巯基琥珀酸（DMSA）和DL-硫辛酸（DL-TA）对金电极进行了表面修饰DL-TA-SAM修饰电极的ECL约为裸电极的5倍，SAM修饰电极的ECL增强是由于带正电的浓度效应Luc〜（2+）离子，防止电致化学发光产物（即N-甲基ac啶酮（NMA）和双电子还原形式的Luc〜（2+）（Luc〜0））在电极表面上的吸附，以及O_2〜（·-）的有效生成。另一方面，m中的ECL量与不含表面活性剂的溶液相比，冰晶溶液增加了约六倍。胶束溶液中增强的ECL主要是由于抑制NMA和不溶于水的Luc〜0在电极表面的吸附所致。

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